Moderate water absorption from OPS fibers and additional dissolution of Al and Si elements due to formation of C–A–S–H gels from limestone inclusion have presented 10% OPS and 25% limestone as the optimum replacement to river sand and coarse granite aggregate, respectively. In ambient curing, 25% limestone presented a 35.23% higher strength while 10% OPS had 11.01% higher strength than control. An escalation to the curing temperature reduced the efficiency of both aggregates, where only 25% limestone was able to produce specimen with 2.34% higher strength than control A supportive analysis from SEM and EDX has also revealed the existence of poly(sialate), poly(sialate-siloxo), poly(sialate-disiloxo) and sialate link in the geopolymer matrix. From this research, the applications of limestone and oil palm shell in geopolymer concrete have presented a nurturing result, particularly as the alternative aggregates in ambient-cured application.